• Search Research Projects
  • Search Researchers
  • How to Use
  1. Back to previous page

Synthesis of ferroelectric perovskite oxynitride with perfect trans-anion order and its application for photovoltaic energy conversion

Research Project

Project/Area Number 19K22227
Research Category

Grant-in-Aid for Challenging Research (Exploratory)

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 36:Inorganic materials chemistry, energy-related chemistry, and related fields
Research InstitutionThe University of Tokyo

Principal Investigator

HIROSE Yasushi  東京大学, 大学院理学系研究科(理学部), 准教授 (50399557)

Project Period (FY) 2019-06-28 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥6,500,000 (Direct Cost: ¥5,000,000、Indirect Cost: ¥1,500,000)
Fiscal Year 2020: ¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000)
Fiscal Year 2019: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Keywords機能性薄膜材料 / 酸窒化物 / 強誘電体 / アニオン配列 / エピタキシャル成長 / 太陽電池 / 光起電力効果 / エピタキシャル薄膜 / エピタキシャル薄膜Å / 光電変換 / 複合アニオン化合物 / 薄膜 / 配位化学
Outline of Research at the Start

強誘電体の光起電力効果を用いた光電変換素子は、高効率太陽電池などへの応用が期待されているが、可視光の利用効率が低い。本研究では可視光を高効率に利用可能な狭バンドギャップの強誘電体薄膜の開発に取り組む。具体的には、顔料や光触媒などに応用されているペロブスカイト酸窒化物(SrTaO2NやLaTiO2N)に注目する。これらの結晶は、TiやTaイオン周囲のOとNの配列を最安定なcis型から準安定なtrans型に変えることで強誘電性を示すと予想されている。本研究では、熱力学的に非平衡な薄膜成長プロセスを駆使し、未だ合成例のない完全trans型配列をもつペロブスカイト酸窒化物強誘電体の合成に挑戦する。

Outline of Final Research Achievements

The synthesis of perovskite oxynitride thin films with trans-type anion arrangement, a candidate for narrow-bandgap ferroelectric material, was studied. Although it was theoretically predicted that A3+B4+O2N-type oxynitrides would stabilize the trans-type arrangement with charge-neutral AN and BO2 planes, no increase in the trans-type arrangement in the synthesized thin films was confirmed. Depth-profile analysis of the N modulation-doped thin films revealed that the diffusion of N in the crystals must be suppressed by low-temperature growth. As another approach, Sn2+ with electron lone pairs was introduced into the A site, which enhances the tetragonal distortion stabilizing the trans-type arrangement. However, the synthesis of such compounds was difficult due to the desorption of SnNx. It was concluded that a solid-phase epitaxy, which can suppress nitride desorption, is promising.

Academic Significance and Societal Importance of the Research Achievements

目標としていた完全trans型ペロブスカイト酸窒化物の合成には至らなかったが、課題(酸窒化物結晶中のアニオン拡散および熱力学的に不安定な窒化物の分解脱離)とその解決に向けた方策を明らかにした。また、酸化物/酸窒化物人工超格子の合成、エピタキシャル酸化物薄膜を前駆体に用いたトポタクティック窒化反応、逆光電子ホログラフィーによる単結晶薄膜中のアニオン配列評価といった新たな技術の開発に成功した。

Report

(4 results)
  • 2021 Annual Research Report   Final Research Report ( PDF )
  • 2020 Research-status Report
  • 2019 Research-status Report
  • Research Products

    (18 results)

All 2022 2021 2020 2019

All Journal Article (6 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 6 results,  Open Access: 3 results) Presentation (11 results) (of which Int'l Joint Research: 1 results,  Invited: 2 results) Book (1 results)

  • [Journal Article] Installation of TOF-E telescope ERDA in UTTAC at the University of Tsukuba: Analysis of metal-nitride-based multi-layer coatings on glasses2021

    • Author(s)
      Sugisawa Y.、Harayama I.、Takimoto Y.、Wakasugi T.、Hirose Y.、Hasegawa T.、Ishii S.、Sekiba D.
    • Journal Title

      Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms

      Volume: 503 Pages: 68-74

    • DOI

      10.1016/j.nimb.2021.07.006

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] X-ray Fluorescence Holography Measurement of Oxynitride Thin Film of CaTaO<sub>2</sub>N2021

    • Author(s)
      Yamamoto Yuta、Kimura Koji、Ang Artoni Kevin R.、Hirose Yasushi、Hayashi Kouichi
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 19 Issue: 0 Pages: 99-103

    • DOI

      10.1380/ejssnt.2021.99

    • NAID

      130008104904

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Electron localization induced by intrinsic anion disorder in a transition metal oxynitride2021

    • Author(s)
      Oka Daichi、Hirose Yasushi、Nakao Shoichiro、Fukumura Tomoteru、Hasegawa Tetsuya
    • Journal Title

      Communications Physics

      Volume: 4 Issue: 1 Pages: 269-269

    • DOI

      10.1038/s42005-021-00777-z

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Exploring Metastable Oxynitrides by Thin Film Growth Approach2021

    • Author(s)
      Hirose Yasushi、Hasegawa Tetsuya
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 94 Issue: 4 Pages: 1355-1363

    • DOI

      10.1246/bcsj.20210033

    • NAID

      130008037350

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Anion arrangement analysis of oxynitride perovskite thin film with inverse photoelectron holography2021

    • Author(s)
      Yamamoto Y.、Ang A.K.R.、Kimura K.、Matsushita T.、Hirose Y.、Oka D.、Hayashi K.
    • Journal Title

      Journal of Electron Spectroscopy and Related Phenomena

      Volume: 246 Pages: 147018-147018

    • DOI

      10.1016/j.elspec.2020.147018

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] High-Quality Heteroepitaxial Growth of Thin Films of the Perovskite Oxynitride CaTaO2N: Importance of Interfacial Symmetry Matching between Films and Substrates2020

    • Author(s)
      Wakasugi Takuto、Hirose Yasushi、Nakao Shoichiro、Sugisawa Yuki、Sekiba Daiichiro、Hasegawa Tetsuya
    • Journal Title

      ACS Omega

      Volume: 5 Issue: 22 Pages: 13396-13402

    • DOI

      10.1021/acsomega.0c01601

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] CaTaO2N単結晶薄膜光電極のキャリア輸送効率に影響を与える因子の探索とゼロバイアス水分解反応の実現2022

    • Author(s)
      若杉拓人、廣瀬靖、岡田和也、長谷川哲也
    • Organizer
      第129回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 準安定な複合アニオン酸化物の薄膜合成と電子機能の探索2021

    • Author(s)
      廣瀬靖
    • Organizer
      第134回 フロンティア材料研究所学術講演会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Presentation] スズ酸窒化物(SnOxNy)薄膜の電子輸送特性2021

    • Author(s)
      土井 雅人、廣瀬 靖、長谷川 哲也
    • Organizer
      第68回応用物理学会春季学術講演会
    • Related Report
      2020 Research-status Report
  • [Presentation] 化学エッチングによるCaTaO2N単結晶薄膜の欠陥密度評価2021

    • Author(s)
      若杉拓人、廣瀬靖、長谷川哲也
    • Organizer
      第127回触媒討論会
    • Related Report
      2020 Research-status Report
  • [Presentation] パイロクロア型Sn2Ta2O7エピタキシャル薄膜のトポタクティック窒化2021

    • Author(s)
      福本 通孝、廣瀬 靖、土井 雅人、杉澤 悠紀、関場 大一郎、長谷川 哲也
    • Organizer
      第68回応用物理学会春季学術講演会
    • Related Report
      2020 Research-status Report
  • [Presentation] CaTaO2N単結晶薄膜光電極を用いた水分解反応における界面対称性の重要性2020

    • Author(s)
      若杉拓人、廣瀬靖、長谷川哲也
    • Organizer
      第14回 物性科学領域横断研究会
    • Related Report
      2020 Research-status Report
  • [Presentation] CaTaO2Nエピタキシャル薄膜の結晶面方位が水分解光電極特性に与える影響2020

    • Author(s)
      若杉択人、廣瀬靖、熊谷啓、前田和彦、長谷川哲也
    • Organizer
      第125回触媒討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] SrWO3-xNx薄膜の作製とその電子輸送特性2020

    • Author(s)
      丸山敬裕, 近松彰, 廣瀬靖, 片山司, 長谷川哲也
    • Organizer
      第67回 応用物理学会 春季学術講演会
    • Related Report
      2019 Research-status Report
  • [Presentation] Functionalization of oxide-based mixed anion compound thin films2019

    • Author(s)
      Yasushi Hirose
    • Organizer
      Materials Research Meeting 2019 (MRM2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 結晶面方位を制御したCaTaO2N薄膜へのCoOxの光析出と光電極特性への影響2019

    • Author(s)
      若杉 択人、廣瀬 靖、熊谷 啓、前田 和彦、長谷川 哲也
    • Organizer
      第80回応用物理学会秋季学術講演会
    • Related Report
      2019 Research-status Report
  • [Presentation] ) Influence of Crystallographic Orientation on the Activity of Photoelectrochemical Water Splitting with CaTaO2N2019

    • Author(s)
      Takuto WAKASUGI, Yasushi HIROSE, Shoichiro NAKAO, Hiromu KUMAGAI, Kazuhiko MAEDA, Tetsuya HASEGAWA
    • Organizer
      The 13th Pacific Rim Conference of Ceramic Societies (PACRIM13)
    • Related Report
      2019 Research-status Report
  • [Book] 複合アニオン化合物の科学2021

    • Author(s)
      陰山 洋、荻野 拓、長谷川 哲也
    • Total Pages
      264
    • Publisher
      丸善出版
    • ISBN
      9784621306109
    • Related Report
      2020 Research-status Report

URL: 

Published: 2019-07-04   Modified: 2023-01-30  

Information User Guide FAQ News Terms of Use Attribution of KAKENHI

Powered by NII kakenhi